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Our current understanding of Arctic carbonaceous aerosol (CA) is rudimentary and there is a lack of long-term observations for many components, such as organic aerosol (OA), exceptions to this include equivalent black carbon (eBC) and methane sulfonic acid (MSA). To address this, we analyzed long-term measurements of organic carbon (OC), elemental carbon (EC), and source-specific organic tracers from 2017 to 2020 to constrain CA sources in the rapidly changing Arctic. We also used absorption photometer (aethalometer) measurements to constrain equivalent BC from biomass burning (eBCBB) and fossil fuel combustion (eBCFF) using Positive Matrix Factorization (PMF). Our analysis showed that organic tracers are essential to understand Arctic CA sources. For 2017 to 2020, levoglucosan had a bimodal seasonality, with a signal from residential wood combustion (RWC) in the heating season (H-season; November to May) and from wildfires (WF) in the non-heating season (NH-season; June to October), demonstrating a pronounced inter-annual variability in the WF influence. Biogenic secondary organic aerosol (BSOA) species (2-methyltetrols) from isoprene oxidation appeared only in the NH-season, peaking in July to August. Intrusions of warm air masses from Siberia in summer caused three- and ninefold increases in 2-methyltetrols compared to 2017 to 2018, in 2019 and 2020, respectively, warranting investigation of the local vs. the long-range atmospheric transport (LRT) contribution, as certain Arctic vegetation has highly temperature sensitive biogenic volatile organic compounds (BVOC) emission rates. Primary biological aerosol particles (PBAP) tracers (various sugars and sugar-alcohols) were elevated in the NH-season but evolved differently, whereas cellulose was completely decoupled from the other PBAP tracers. Peak levels of most PBAP tracers and of 2-methyltetrols were associated with WF emissions, demonstrating the importance of measuring a broad spectrum of source specific tracers to understand sources and dynamics of CA. Finally, CA seasonality is heavily influenced by long-range atmospheric transport (LRT) episodes, since background levels are extremely low. E.g., we find the OA peak in the NH-season is as strongly influenced by LRT as is EC during Arctic Haze (AH). Source apportionment of CA by Latin Hypercube Sampling (LHS) showed a mixed contribution from RWC (46 %), fossil fuel (FF) sources (27 %), and BSOA (25 %) in the H-season, whereas BSOA (56 %) prevailed over WF (26 %) and FF (15 %) in the NH-season. Source apportionment of eBC by PMF showed that FF combustion dominated eBC (70 ± 2.7 %), whereas RWC (22 ± 2.7 %) was more abundant than WF (8.0 ± 2.9 %). Modeled BC concentrations from FLEXPART attributed an almost equal share to FF (51 ± 3.1 %) and BB. Both FLEXPART and the PMF analysis concluded that RWC is a more important source than WF. However, with a modeled RWC of 30 ± 4.1 % and WF of 19 ± 2.8 %, FLEXPART suggests relatively higher contributions to eBC from these sources. We find that OA (281 ± 106 ng m−3) is a significant fraction of the Arctic PM10 aerosol particle mass, though less than sea salt aerosol (SSA) (682 ± 46.9 ng m−3) and mineral dust (MD) (613 ± 368 ng m−3) as well as typically non-sea-salt sulfate (nssSO42−) (314 ± 62.6 ng m−3), originating mainly from anthropogenic sources in winter and from natural sources in summer. FF combustion was the prevailing source of eBC, whereas RWC made a larger contribution to eBCBB than WF.

The Zeppelin Observatory (78.90° N, 11.88° E) is located on the Zeppelin Mountain at 472 m above sea level on Spitsbergen, the largest island of the Svalbard archipelago. Established in 1989, the observatory is part of the “Ny-Ålesund Research Station” and an important atmospheric measurement site, one of only a few in the high Arctic and as a part of several European and global monitoring programs and research infrastructures, notably the European Monitoring and Evaluation Programme (EMEP), the Arctic Monitoring and Assessment Programme (AMAP), the Global Atmosphere Watch (GAW), the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS), the Advanced Global Atmospheric Gases Experiment (AGAGE) network, and the Integrated Carbon Observation System (ICOS). The observatory is jointly operated by the Norwegian Polar Institute (NPI), Stockholm University and the Norwegian Institute for Air Research (NILU). Here we detail the establishment of the Zeppelin Observatory including historical measurements of atmospheric composition in the European Arctic leading to its construction. We present a history of the measurements at the observatory and review the current state of the European Arctic atmosphere, including results from trends in greenhouse gases, chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs), other traces gases, persistent organic pollutants (POPs) and heavy metals, aerosols and Arctic haze, and atmospheric transport phenomena.

Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes. Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50 % decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2∕3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1. Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AODf, AODc), Ångström exponent (AE), dry surface scattering (SCdry), and absorption (ACdry) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21 % ± 20 % (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from −37 % (MODIS-Terra) to −16 % (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R>0.75), suggesting that the models are capable of capturing spatio-temporal variations in AOD. We find a much larger underestimate in coarse AODc (∼ −45 % ± 25 %) than in fine AODf (∼ −15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AODc bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AODc. Column AEs are underestimated by about 10 % ± 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. +140 % if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment. Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of −35 % ± 25 % and −20 % ± 18 % for SCdry and ACdry, respectively. The larger underestimate of SCdry than ACdry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SCdry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models. Considerable inter-model diversity in the simulated optical properties is often found in regions that are, unfortunately, not or only sparsely covered by ground-based observations. This includes, for instance, the Sahara, Amazonia, central Australia, and the South Pacific. This highlights the need for a better site coverage in the observations, which would enable us to better assess the models, but also the performance of satellite products in these regions. Using fine-mode AOD as a proxy for present-day aerosol forcing estimates, our results suggest that models underestimate aerosol forcing by ca. −15 %, however, with a considerably large interquartile range, suggesting a spread between −35 % and +10 %.

Since 1750, land-use change and fossil fuel combustion has led to a 46% increase in the atmospheric carbon dioxide (CO2) concentrations, causing global warming with substantial societal consequences. The Paris Agreement aims to limit global temperature increases to well below 2°C above preindustrial levels. Increasing levels of CO2 and other greenhouse gases (GHGs), such as methane (CH4) and nitrous oxide (N2O), in the atmosphere are the primary cause of climate change. Approximately half of the carbon emissions to the atmosphere are sequestered by ocean and land sinks, leading to ocean acidification but also slowing the rate of global warming. However, there are significant uncertainties in the future global warming scenarios due to uncertainties in the size, nature, and stability of these sinks. Quantifying and monitoring the size and timing of natural sinks and the impact of climate change on ecosystems are important information to guide policy-makers’ decisions and strategies on reductions in emissions. Continuous, long-term observations are required to quantify GHG emissions, sinks, and their impacts on Earth systems. The Integrated Carbon Observation System (ICOS) was designed as the European in situ observation and information system to support science and society in their efforts to mitigate climate change. It provides standardized and open data currently from over 140 measurement stations across 12 European countries. The stations observe GHG concentrations in the atmosphere and carbon and GHG fluxes between the atmosphere, land surface, and the oceans. This article describes how ICOS fulfills its mission to harmonize these observations, ensure the related long-term financial commitments, provide easy access to well-documented and reproducible high-quality data and related protocols and tools for scientific studies, and deliver information and GHG-related products to stakeholders in society and policy.

We present 18 years (2001–2018) of aerosol measurements: organic- and elemental carbon (OC and EC), organic tracers (levoglucosan, arabitol, mannitol, trehalose, glucose, 2-methyltetrols), trace elements and ions – at the Birkenes Observatory (Southern Norway), a site representative of the Northern European region. The OC / EC (2001–2018) and the levoglucosan (2008–2018) time series are the longest in Europe, with OC / EC available for the PM10, PM2.5 (fine) and PM10-2.5 (coarse) size fractions, providing the opportunity for a nearly two-decade long assessment. Using positive matrix factorisation (PMF) we identify six carbonaceous aerosol sources at Birkenes: Mineral dust dominated (MIN), traffic/industry-like (TRA/IND), short range transported biogenic secondary organic aerosol (BSOASRT), primary biological aerosol particles (PBAP), biomass burning (BB), and ammonium nitrate dominated (NH4NO3), and one low carbon fraction, sea salt (SS). We observed significant (p 10 (−3.9 % yr−1) and PM2.5 (−4.2 % yr−1), and a smaller decline in levoglucosan (−2.8 % yr−1), suggesting that OC / EC from traffic and industry is decreasing, while abatement of OC / EC from biomass burning has been slightly less successful. EC abatement of anthropogenic sources is further supported by decreasing EC fractions in PM2.5 (−4.0 % yr−1) and PM10 (−4.7 % yr−1). PMF apportioned 72 % of EC to fossil fuel sources, further supported by PMF applied to absorption photometer data, which yielded a two-factor solution with a low aerosol Ångstrøm exponent (AAE = 0.93) fraction assumed to be equivalent black carbon from fossil fuel combustion (eBCff), contributing 78 % to eBC mass. The higher AAE fraction (AAE = 2.04) is likely eBC from BB (eBCbb). Source receptor model calculations (FLEXPART) showed that Continental Europe and western Russia were the main source regions both of elevated eBCbb and eBCff. A relative increase in the OC fraction in PM2.5 (+3.2 % yr−1) and PM10 (+2.3 % yr−1) underscores the importance of biogenic sources at Birkenes (BSOA and PBAP), which were higher in the vegetative season and dominated both fine (53 %) and coarse (78 %) OC. Furthermore, 77–91 % of OC in PM2.5, PM10-2.5 and PM10 was attributed to biogenic sources in summer vs. 22–37 % in winter. The coarse fraction had the highest share of biogenic sources regardless of season and was dominated by PBAP, except in winter. Our results show a shift in aerosol composition at Birkenes and thus also in the relative source contributions. The need for diverse off-line and on-line carbonaceous aerosol speciation to understand carbonaceous aerosol sources, including their seasonal, annual, and long-term variability has been demonstrated.

Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the present day modelling of aerosol optical properties has been assessed using simulated data representative for the year 2010, from 14 global aerosol models participating in the Phase III Control experiment. The model versions are close or equal to those used for CMIP6 and AerChemMIP and inform also on bias in state of the art ESMs. Modelled column optical depths (total, fine and coarse mode AOD) and Angstrom Exponents (AE) were compared both with ground based observations from the Aerosol Robotic Network (AERONET, version 3) as well as space based observations from AATSR-SU instruments. In addition, the modelled AODs were compared with MODIS (Aqua and Terra) data and a satellite AOD data-set (MERGED-FMI) merged from 12 different individual AOD products. Furthermore, for the first time, the modelled near surface scattering (under dry conditions) and absorption coefficients were evaluated against measurements made at low relative humidity at surface in-situ GAW sites. Statistics are based mainly on normalised mean biases and Pearson correlation coefficients from colocated model and observation data in monthly resolution. Hence, the results are mostly representative for the regions covered by each of the observation networks. Model biases established against satellite data yield insights into remote continental areas and oceans, where ground-based networks lack site coverage. The satellite data themselves are evaluated against AERONET observations, to test our aggregation and re-gridding routines, suggesting relative AOD biases of −5 %, −6 %, +9 % and +18 % for AATSR-SU, MERGED-FMI, MODIS-aqua and MODIS-terra, respectively, with high correlations exceeding 0.8. Biases of fine and coarse AOD and AE in AATSR are found to be +2 %, −16 % and +14.7 % respectively, at AERONET sites, with correlations of the order of 0.8. The AeroCom MEDIAN and most of the participating models underestimate the optical properties investigated, relative to remote sensing observations. AERONET AOD is underestimated by 21 % ± 17 %. Against satellite data, the model AOD biases range from −38 % (MODIS-terra) to −17 % (MERGED-FMI). Correlation coefficients of model AODs with AERONET, MERGED-FMI and AATSR-SU are high (0.8–0.9) and slightly lower against the two MODIS data-sets (0.6–0.8). Investigation of fine and coarse AODs from the MEDIAN model reveals biases of −10% ± 20 % and −41 % ± 29 % against AERONET and −13 % and −24 % against AATSR-SU, respectively. The differences in bias against AERONET and AATSR-SU are in agreement with the established satellite bias against AERONET. These results indicate that most of the AOD bias is due to missing coarse AOD in the regions covered by these observations. Underestimates are also found when comparing the models against the surface GAW observations, showing AeroCom MEDIAN mean bias and inter-model variation of −44 % ± 22 % and −32 % ± 34 % for scattering and absorption coefficients, respectively. Dry scattering shows higher underestimation than AOD at ambient relative humidity and is in agreement with recent findings that suggest that models tend to overestimate scattering enhancement due to hygroscopic growth. Broadly consistent negative bias in AOD and scattering suggest a general underestimate in aerosol effects in current global aerosol models. The large diversity in the surface absorption results suggests differences in the model treatment of light absorption by black carbon (BC), dust (DU) and to a minor degree, organic aerosol (OA). Considerable diversity is found among the models in the simulated near surface absorption coefficients, particularly in regions associated with dust (e.g. Sahara, Tibet), biomass burning (e.g. Amazonia, Central Australia) and biogenic emissions (e.g. Amazonia). Regions associated with high anthropogenic BC emissions such as China and India exhibit comparatively good agreement for all models. Evaluation of modelled column AEs shows an underestimation of 9 % ± 24 % against AERONET and −21 % against AATSR-SU. This suggests that overall, models tend to overestimate particle size, with implications for lifetime and radiative transfer calculations. An investigation of modelled emissions, burdens and lifetimes, mass-specific-extinction coefficients (MECs) and optical depths (ODs) for each species and model reveals considerable diversity in most of these parameters. These are discussed in detail for each model individually. Inter-model spread of aerosol species lifetime appears to be similar to that of mass extinction coefficients, suggesting that AOD uncertainties are still associated to a broad spectrum of parameterised aerosol processes.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Aerosol particles are essential constituents of the Earth’s atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence time resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in-situ near-surface segment of the atmospheric observations system. This paper will provide the widest effort so far to document variability of climate-relevant in-situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High quality data from more than 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single scattering albedo and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information including data provision procedures, quality control and analysis, data policy and usage of the ground-based aerosol measurements network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully-characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.

The profound changes in global SO_2 emissions over the last decades have affected atmospheric composition on a regional and global scale with large impact on air quality, atmospheric deposition and the radiative forcing of sulfate aerosols. Reproduction of historical atmospheric pollution levels based on global aerosol models and emission changes is crucial to prove that such models are able to predict future scenarios. Here, we analyze consistency of trends in observations of sulfur components in air and precipitation from major regional networks and estimates from six different global aerosol models from 1990 until 2015. There are large interregional differences in the sulfur trends consistently captured by the models and observations, especially for North America and Europe. Europe had the largest reductions in sulfur emissions in the first part of the period while the highest reduction came later in North America and East Asia. The uncertainties in both the emissions and the representativity of the observations are larger in Asia. However, emissions from East Asia clearly increased from 2000 to 2005 followed by a decrease, while in India a steady increase over the whole period has been observed and modelled. The agreement between a bottom-up approach, which uses emissions and process-based chemical transport models, with independent observations gives an improved confidence in the understanding of the atmospheric sulfur budget., 論文

Accepted manuscript version, licensed CC BY-NC-ND 4.0. We investigate methane seepage on the shallow shelf west of Svalbard during three consecutive years, using discrete sampling of the water column, echosounder-based gas flux estimates, water mass properties, and numerical dispersion modelling. The results reveal three distinct hydrographic conditions in spring and summer, showing that the methane content in the water column is controlled by a combination of free gas seepage intensity and lateral water mass movements, which disperse and displace dissolved methane horizontally away from the seeps. Horizontal dispersion and displacement of dissolved methane are promoted by eddies originating from the West Spitsbergen Current and passing over the shallow shelf, a process that is more intense in winter and spring than in the summer season. Most of the methane injected from seafloor seeps resides in the bottom layer even when the water column is well mixed, implying that the controlling effect of water column stratification on vertical methane transport is small. Only small concentrations of methane are found in surface waters, and thus the escape of methane into the atmosphere above the site of seepage is also small. The magnitude of the sea to air methane flux is controlled by wind speed, rather than by the concentration of dissolved methane in the surface ocean.

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.

International audience; Anthropogenic mercury emissions are transported through the atmosphere as gaseous elemental mercury (Hg(0)) before they are deposited to Earth’s surface. Strong seasonality in atmospheric Hg(0) concentrations in the Northern Hemisphere has been explained by two factors: anthropogenic Hg(0) emissions are thought to peak in winter due to higher energy consumption, and atmospheric oxidation rates of Hg(0) are faster in summer. Oxidation-driven Hg(0) seasonality should be equally pronounced in the Southern Hemisphere, which is inconsistent with observations of constant year-round Hg(0) levels. Here, we assess the role of Hg(0) uptake by vegetation as an alternative mechanism for driving Hg(0) seasonality. We find that at terrestrial sites in the Northern Hemisphere, Hg(0) co-varies with CO$_2$, which is known to exhibit a minimum in summer when CO$_2$ is assimilated by vegetation. The amplitude of seasonal oscillations in the atmospheric Hg(0) concentration increases with latitude and is larger at inland terrestrial sites than coastal sites. Using satellite data, we find that the photosynthetic activity of vegetation correlates with Hg(0) levels at individual sites and across continents. We suggest that terrestrial vegetation acts as a global Hg(0) pump, which can contribute to seasonal variations of atmospheric Hg(0), and that decreasing Hg(0) levels in the Northern Hemisphere over the past 20 years can be partly attributed to increased terrestrial net primary production.

An edited version of this paper was published by AGU. Copyright (2018) American Geophysical Union. Ericson, Y., Falck, E., Chierici, M., Fransson, A., Kristiansen, S., Platt, S.M., ... Myhre, C.L. (2018). Temporal variability in surface water pCO2 in Adventfjorden (West Spitsbergen) with emphasis on physical and biogeochemical drivers. Journal of Geophysical Research - Oceans, 123, 4888-4905. https://doi.org/10.1029/2018JC014073. To view the published open abstract, go to https://doi.org/10.1029/2018JC014073. Seasonal and interannual variability in surface water partial pressure of CO2 (pCO2) and air‐sea CO2 fluxes from a West Spitsbergen fjord (IsA Station, Adventfjorden) are presented, and the associated driving forces are evaluated. Marine CO2 system data together with temperature, salinity, and nutrients, were collected at the IsA Station between March 2015 and June 2017. The surface waters were undersaturated in pCO2 with respect to atmospheric pCO2 all year round. The effects of biological activity (primary production/respiration) followed by thermal forcing on pCO2 were the most important drivers on a seasonal scale. The ocean was a sink for atmospheric CO2 with annual air‐sea CO2 fluxes of −36 ± 2 and −31 ± 2 g C·m−2·year−1 for 2015–2016 and 2016–2017, respectively, as estimated from the month of April. Waters of an Arctic origin dominated in 2015 and were replaced in 2016 by waters of a transformed Atlantic source. The CO2 uptake rates over the period of Arctic origin waters were significantly higher (2 mmol C·m−2·day−1) than the rates of the Atlantic origin waters of the following year.

Methane (CH4) is a powerful greenhouse gas. Its atmospheric mixing ratios have been increasing since 2005. Therefore, quantification of CH4 sources is essential for effective climate change mitigation. Here we report observations of the CH4 mixing ratios measured at the Zeppelin Observatory (Svalbard) in the Arctic and aboard the research vessel (RV) Helmer Hanssen over the Arctic Ocean from June 2014 to December 2016, as well as the long-term CH4 trend measured at the Zeppelin Observatory from 2001 to 2017. We investigated areas over the European Arctic Ocean to identify possible hotspot regions emitting CH4 from the ocean to the atmosphere, and used state-of-the-art modelling (FLEXPART) combined with updated emission inventories to identify CH4 sources. Furthermore, we collected air samples in the region as well as samples of gas hydrates, obtained from the sea floor, which we analysed using a new technique whereby hydrate gases are sampled directly into evacuated canisters. Using this new methodology, we evaluated the suitability of ethane and isotopic signatures (δ13C in CH4) as tracers for ocean-to-atmosphere CH4 emission. We found that the average methane / light hydrocarbon (ethane and propane) ratio is an order of magnitude higher for the same sediment samples using our new methodology compared to previously reported values, 2379.95 vs. 460.06, respectively. Meanwhile, we show that the mean atmospheric CH4 mixing ratio in the Arctic increased by 5.9±0.38 parts per billion by volume (ppb) per year (yr−1) from 2001 to 2017 and ∼8 pbb yr−1 since 2008, similar to the global trend of ∼ 7–8 ppb yr−1. Most large excursions from the baseline CH4 mixing ratio over the European Arctic Ocean are due to long-range transport from land-based sources, lending confidence to the present inventories for high-latitude CH4 emissions. However, we also identify a potential hotspot region with ocean–atmosphere CH4 flux north of Svalbard (80.4∘ N, 12.8∘ E) of up to 26 nmol m−2 s−1 from a large mixing ratio increase at the location of 30 ppb. Since this flux is consistent with previous constraints (both spatially and temporally), there is no evidence that the area of interest north of Svalbard is unique in the context of the wider Arctic. Rather, because the meteorology at the time of the observation was unique in the context of the measurement time series, we obtained over the short course of the episode measurements highly sensitive to emissions over an active seep site, without sensitivity to land-based emissions.

The “double CO2” experiment has become a standard experiment in climate science, and a convenient way of comparing the sensitivity of different climate models. Double CO2 was first used by Arrhenius in the 19th century and in the classic paper by Manabe and Wetherald, published 50 years ago, which marked the start of the modern era of climate modeling. Doubling CO2 now has an iconic role in climate research. The equilibrium climate sensitivity (ECS) is defined as the global-mean surface temperature change resulting from a doubling of CO2, which is a headline result in Intergovernmental Panel on Climate Change (IPCC) assessments. In its most recent assessment IPCC concluded that the ECS “is likely in the range 1.5 to 4.5oC”. We show that we are now halfway to doubling of CO2 since pre-industrial times in terms of radiative forcing, but not in concentration.

Over the past decades, the geographical distribution of emissions of substances that alter the atmospheric energy balance has changed due to economic growth and pollution regulations. Here, we show the resulting changes to aerosol and ozone abundances and their radiative forcing, using recently updated emission data for the period 1990–2015, as simulated by seven global atmospheric composition models. The models broadly reproduce the large-scale changes in surface aerosol and ozone based on observations (e.g., −1 to −3 %/yr in aerosols over US and Europe). The global mean radiative forcing due to ozone and aerosols changes over the 1990–2015 period increased by about +0.2 W m−2, with approximately 1/3 due to ozone. This increase is stronger positive than reported in IPCC AR5. The main reason for the increased positive radiative forcing of aerosols over this period is the substantial reduction of global mean SO2 emissions which is stronger in the new emission inventory compared to the IPCC, and higher black carbon emissions.

International audience; Peng et al. (1) conclude that a fast increase in the mass absorption cross-section (MAC) of black carbon (BC) in urban environments leads to significantly increased estimates of the BC radiative forcing (RF). Their chamber measurements are highly valuable and complement observations performed in ambient conditions, but their "enhancement factor" relative to an unspec-ified baseline may not be directly comparable to values used or simulated in global aerosol models. MAC, a key parameter in our understanding of the net BC climate impact, is indeed a more relevant quantity to examine. A fast MAC enhancement in polluted environments as the BC gets coated with organic and inorganic species is consistent with recent findings (2, 3). Global models used in AeroCom [table S1 in Peng et al. (1), ref. 4] have an average MAC of ∼8 m 2 ·g −1 at 550 nm. This value is reflecting reported measurements, although there is a large spatial and seasonal variability in ambient MAC for aged particles, with values of ∼10 m 2 ·g −1 at a rural Northern Chinese site (2) (at 678 nm); 6-14 m 2 ·g −1 at rural, urban, and high-altitude Indian locations (5) (at 678 nm); and ∼6 m 2 ·g −1 at an Arctic site (6) (at 522 nm). Coating of BC by soluble species not only enhances absorption of solar radiation but also reduces the BC atmospheric lifetime (7). Fig. 1 shows an offset between the increase in average MAC value with faster BC aging and an overall shorter BC lifetime, resulting in a near-constant BC aerosol absorption optical depth and RF with aging time. Furthermore, current global aerosol models frequently have a too long BC lifetime and consequently overestimate BC concentrations downwind from source regions (8). According to Peng et al. (1), their BC absorption enhancement factor of 2.4 is also an upper bound, only reached after 5 (Beijing) to 18 (Houston) h, and possibly longer in cleaner environments. Such timescales are not small compared with the BC atmospheric lifetime of 3-5 d, especially considering that dilution effects may lengthen the aging timescale in the real atmosphere compared with the static chamber measurements performed by Peng et al. It is unclear how representative these measurements are for global and annual averages, but we know that generalizations can introduce serious errors due to spatial and temporal sampling issues (9). This implies that a simple scaling of the BC RF by the absorption enhancement factor measured by Peng et al.-as performed by the authors in their table S1 and figure 4, and extended in the commentary (10)-is overly simplistic. In conclusion, although we welcome the advances made by Peng et al., their conclusion of a +0.45 [0.21-0.80] W·m −2 additional RF due to a large BC enhancement factor is premature. The jury is still out on the question of the net climate impact of BC and how much climate cobenefit will result from the necessary mitigation of BC emissions. Reducing the uncertainty on the BC forcing requires better constraining BC MAC and atmospheric lifetime in global aerosol models.

Large-scale climate patterns influenced temperature and weather patterns around the globe in 2011. In particular, a moderate-to-strong La Niña at the beginning of the year dissipated during boreal spring but reemerged during fall. The phenomenon contributed to historical droughts in East Africa, the southern United States, and northern Mexico, as well the wettest two-year period (2010-11) on record for Australia, particularly remarkable as this follows a decade-long dry period. Precipitation patterns in South America were also influenced by La Niña. Heavy rain in Rio de Janeiro in January triggered the country's worst floods and landslides in Brazil's history. The 2011 combined average temperature across global land and ocean surfaces was the coolest since 2008, but was also among the 15 warmest years on record and above the 1981-2010 average. The global sea surface temperature cooled by 0.1°C from 2010 to 2011, associated with cooling influences of La Niña. Global integrals of upper ocean heat content for 2011 were higher than for all prior years, demonstrating the Earth's dominant role of the oceans in the Earth's energy budget. In the upper atmosphere, tropical stratospheric temperatures were anomalously warm, while polar temperatures were anomalously cold. This led to large springtime stratospheric ozone reductions in polar latitudes in both hemispheres. Ozone concentrations in the Arctic stratosphere during March were the lowest for that period since satellite records began in 1979. An extensive, deep, and persistent ozone hole over the Antarctic in September indicates that the recovery to pre-1980 conditions is proceeding very slowly. Atmospheric carbon dioxide concentrations increased by 2.10 ppm in 2011, and exceeded 390 ppm for the first time since instrumental records began. Other greenhouse gases also continued to rise in concentration and the combined effect now represents a 30% increase in radiative forcing over a 1990 baseline. Most ozone depleting substances continued to fall. The global net ocean carbon dioxide uptake for the 2010 transition period from El Niño to La Niña, the most recent period for which analyzed data are available, was estimated to be 1.30 Pg C yr-1, almost 12% below the 29-year long-term average. Relative to the long-term trend, global sea level dropped noticeably in mid-2010 and reached a local minimum in 2011. The drop has been linked to the La Nina conditions that prevailed throughout much of 2010-11. Global sea level increased sharply during the second half of 2011. Global tropical cyclone activity during 2011 was wellbelow average, with a total of 74 storms compared with the 1981-2010 average of 89. Similar to 2010, the North Atlantic was the only basin that experienced abovenormal activity. For the first year since the widespread introduction of the Dvorak intensity-estimation method in the 1980s, only three tropical cyclones reached Category 5 intensity level-all in the Northwest Pacific basin. The Arctic continued to warm at about twice the rate compared with lower latitudes. Below-normal summer snowfall, a decreasing trend in surface albedo, and aboveaverage surface and upper air temperatures resulted in a continued pattern of extreme surface melting, and net snow and ice loss on the Greenland ice sheet. Warmerthan- normal temperatures over the Eurasian Arctic in spring resulted in a new record-low June snow cover extent and spring snow cover duration in this region. In the Canadian Arctic, the mass loss from glaciers and ice caps was the greatest since GRACE measurements began in 2002, continuing a negative trend that began in 1987. New record high temperatures occurred at 20 m below the land surface at all permafrost observatories on the North Slope of Alaska, where measurements began in the late 1970s. Arctic sea ice extent in September 2011 was the second-lowest on record, while the extent of old ice (four and five years) reached a new record minimum that was just 19% of normal. On the opposite pole, austral winter and spring temperatures were more than 3°C above normal over much of the Antarctic continent. However, winter temperatures were below normal in the northern Antarctic Peninsula, which continued the downward trend there during the last 15 years. In summer, an all-time record high temperature of -12.3°C was set at the South Pole station on 25 December, exceeding the previous record by more than a full degree. Antarctic sea ice extent anomalies increased steadily through much of the year, from briefly setting a record low in April, to well above average in December. The latter trend reflects the dispersive effects of low pressure on sea ice and the generally cool conditions around the Antarctic perimeter. © 2012 American Meteorological Society.

Large sets of filtered actinometer, filtered pyrheliometer and Sun photometer measurements have been carried out over the past 30 years by various groups at different Arctic and Antarctic sites and for different time periods. They were examined to estimate ensemble average, long-term trends of the summer background aerosol optical depth AOD(500 nm) in the polar regions ( omitting the data influenced by Arctic haze and volcanic eruptions). The trend for the Arctic was estimated to be between -1.6% and -2.0% per year over 30 years, depending on location. No significant trend was observed for Antarctica. The time patterns of AOD( 500 nm) and angstrom ngstrom's parameters a and beta measured with Sun photometers during the last 20 years at various Arctic and Antarctic sites are also presented. They give a measure of the large variations of these parameters due to El Chichon, Pinatubo, and Cerro Hudson volcanic particles, Arctic haze episodes most frequent in winter and spring, and the transport of Asian dust and boreal smokes to the Arctic region. Evidence is also shown of marked differences between the aerosol optical parameters measured at coastal and high-altitude sites in Antarctica. In situ optical and chemical composition parameters of aerosol particles measured at Arctic and Antarctic sites are also examined to achieve more complete information on the multimodal size distribution shape parameters and their radiative properties. A characterization of aerosol radiative parameters is also defined by plotting the daily mean values of a as a function of AOD( 500 nm), separately for the two polar regions, allowing the identification of different clusters related to fifteen aerosol classes, for which the spectral values of complex refractive index and single scattering albedo were evaluated.